Spin Physics of Excitons in Colloidal Nanocrystals

We present a review of spin-dependent properties of excitons in semiconductor colloidal nanocrystals. The photoluminescences (PL) properties of neutral and charged excitons (trions) are compared. The mechanisms and the polarization of radiative recombination of a “dark” (spin-forbidden) exciton that determines the low-temperature PL of colloidal nanocrystals are discussed in detail. The radiative recombination of a dark exciton becomes possible as a result of simultaneous flips of the surface spin and electron spin in a dark exciton that leads to admixture of bright exciton states. This recombination mechanism is effective in the case of a disordered state of the spin system and is suppressed if the polaron ferromagnetic state forms. The conditions and various mechanisms of formation of the spin polaron state and possibilities of its experimental detection are discussed. The experimental and theoretical studies of magnetic field-induced circular polarization of PL in ensembles of colloidal nanocrystals are reviewed.     

Observation of charged excitons in hole-doped carbon nanotubes using photoluminescence and absorption spectroscopy

We report the first observation of trions (charged excitons), three-particle bound states consisting of one electron and two holes, in hole-doped carbon nanotubes at room temperature. When p-type dopants are added to carbon nanotube solutions, the photoluminescence and absorption peaks of the trions appear far below the E11 bright exciton peak, regardless of the dopant species. The unexpectedly large energy separation between the bright excitons and the trions is attributed to the strong electron-hole exchange interaction in carbon nanotubes.     

Optical orientation and spin relaxation of resident electrons in n-doped InAs/GaAs self-assembled quantum dots

We report on optical orientation of electrons in n-doped InAs/GaAs quantum dots. Under non-resonant cw optical pumping, we measure a negative circular polarization of the luminescence of charged excitons (or trions) at low temperature (T=10 K). The dynamics of the recombination and of the circular polarization is studied by time-resolved spectroscopy. We discuss a simple theoretical model for the trion relaxation, that accounts for this remarkable polarization reversal. The interpretation relies on the bypass of Pauli blocking allowed by the anisotropic electron–hole exchange. Eventually, the spin relaxation time of doping electrons trapped in quantum dots is measured by a non-resonant pump–probe experiment.     

Stark effect of negatively and positively charged excitons in semiconductor quantum wells

We study the effect of an electric field applied normal to the layers on the binding energy of charged excitons (or trions) in GaAs quantum wells. We find that, in contrast to the neutral exciton, their binding energy is sharply reduced by modest electric fields. The effect is stronger for the positively charged exciton than the negatively charged one. The ionisation of the excess carrier is explained by the field-induced polarisation of the electron and hole subband wave functions.     

Screening by composite charged particles: the case of quantum well trions

We investigate the screening properties of a two-dimensional gas of charged excitons (trions). In a first approach to this complex problem, we determine the Hartree response of these composite charged particles within a random phase approximation, showing the effect of the trion internal structure. Only in the long wave-length limit, trions behave as point charges with mass equal to the sum of the three particle components. For finite wave-vectors, the trion screening strongly deviate from the point charge behavior and can even vanish completely at a nodal wave-vector, due to a compensation between the contribution of the two electrons and the hole within a trion. Predictions are presented for the screening of a Coulomb potential, the scattering by charged impurities and the properties of trionic plasmons.     

Stabilization energies of charged multiexciton complexes calculated at configuration interaction level

Recombination and stabilization energies of multiexcitons confined in positively and negatively charged semiconductor InGaAs/GaAs quantum dot (QD) samples have been studied by employing large-scale configuration interaction (CI) calculations. The CI calculations show that at most six electrons or two holes can be confined in the QD. Multiply charged multiexciton complexes with up to five excess electrons or two excess holes are also found to be stable, even when a few electron–hole pairs are present in the QD. The chemical potential functions for charged QD samples do not possess the pronounced stepped form as obtained for the corresponding neutral multiexciton complexes. The negatively and the positively charged excitons (negative and positive trions) lie lower in energy as compared to a neutral exciton and a single non-interacting charge carrier in the lowest single-particle state of another quantum dot. The other charged multiexciton complexes studied are not confined with respect to the corresponding neutral multiexciton and a non-interacting charge carrier. To include the contributions from the heavy-hole light-hole (HH–LH) coupling, a perturbative treatment of the band-mixing effects was implemented. The perturbation-theory calculations show that the HH–LH coupling does not shift the energies in the present InGaAs/GaAs QD sample.     

Excitons and multi-exciton complexes bound to a two-dimensional hole layer at a silicon surface: the Kondo effect,the Coulomb blockade and a negative photoconductivity

The recombination radiation line of surface excitons and the recombination radiation line of multi-exciton complexes bound to a two-dimensional hole layer are observed in luminescence spectra of [100] silicon metal–oxide–semiconductor structures at low two-dimensional hole density. The circular polarization of these two lines in a transverse magnetic field is defined by the average electron spin. The hole spin contribution to the circular polarization is very small due to Kondo spin correlations of holes in the excitons and complexes and holes in the two-dimensional hole layer. The Coulomb blockade excludes a direct contribution of the complexes to a surface photoconductivity. Moreover, a significant negative photoconductivity of the two-dimensional holes is observed at high excitation levels, presumably as a result of the quantum scattering of the two-dimensional holes by the complexes. A shell model of surface multi-exciton complexes is introduced.     

自旋极化度对GaAs量子阱中吸收饱和效应与载流子复合动力学的影响研究

本文研究了(001) GaAs量子阱薄膜中重空穴激子近共振抽运-探测的载流子自旋弛豫动力学, 发现载流子的自旋极化对传统的线偏振光吸收饱和效应和载流子复合动力学都有影响. 进一步的抽运流依赖的自旋弛豫和复合动力学研究表明, 自旋极化对线偏振光的吸收饱和效应的影响随抽运流降低而变弱. 在低激发流时, 自旋极化对线偏振吸收饱和效应的影响才可忽略. 然而, 又显现出自旋极化对复合动力学的影响. 分析表明复合动力学的自旋极化依赖性起源于重空穴激子形成浓度的自旋极化依赖性. 复合动力学的自旋极化依赖性表明自旋弛豫时间计算中所涉及的复合时间应该使用自旋极化载流子的复合时间. 基于二维质量作用定律的激子浓度计算表明, 库仑屏蔽效应对激子形成的影响在较低激发载流子浓度下可以忽略.     

Charged and neutral biexciton–exciton cascade in a single quantum dot within a photonic bandgap

We investigate the recombination dynamics of positively charged and neutral biexcitons and excitons in a single InAs/GaAs quantum dot (QD) within a two-dimensional (2D) photonic bandgap (PBG). The 2D PBG makes the exciton lifetime four times longer and enhances photon-extraction efficiency compared to those without the PBG. Photon cross-correlation measurements demonstrate the cascade emissions of both charged and neutral biexcitons–excitons from the same QD. In the charged case, a hole in the p-shell relaxes into the s-shell between the cascade, and the corresponding transition is confirmed based on the spin configuration. The long exciton lifetime with the PBG helps us to reveal the spin dynamics that did not clearly appear in intrinsic QDs.     

Effective scatterings between electrons,excitons and trions

The final goal of this paper is to derive the effective scattering ruling the time evolution of two semiconductor trions using the many-body formalism for composite fermions we have just proposed. However, to understand the importance of the particle composite nature, their bosonic/fermionic character and their overall charge, we also report on scatterings between free electrons, excitons and trions. This leads us to identify the form factors associated to direct processes involving excitons and trions. For transitions between ground states, these form factors reduce to zero and one respectively, in the small momentum transfer limit.     

Exciton-electron interaction in quantum wells with a two dimensional electron gas of low density

II–VI quantum-well structures containing a 2DEG of low density have been investigated by means of polarized photoluminescence, photoluminescence excitation and reflectivity in external magnetic fields up to 20 T. The spin splittings of the exciton X and the negatively charged exciton X ⁻ are measured as a function of the magnetic field strength. The behavior of the magnetic-field-induced polarization degree of the luminescence line related to X ⁻ demonstrates the formation process of negatively charged excitons from excitons and free carriers polarized by the external magnetic field. We have determined the binding energies of the trion formed either with the heavy-hole or the light-hole exciton. The optically detected magnetic resonance (ODMR) technique was applied for the first time to study the optical transition processes in a nanosecond timescale. The electron ODMR was observed with the detection on either the direct exciton or the negatively charged exciton X. Further evidence for the interaction of excitons with the electrons of the two-dimensional gas are demonstrated by a combined exciton-cyclotron resonance line observed in reflectivity and luminescence excitation, shake-up processes observed in photoluminescence, as well as inelastic and spin-dependent scattering processes. Fiz. Tverd. Tela (St. Petersburg) 41, 831–836 (May 1999) Published in English in the original Russian journal. Reproduced here with stylistic changes by the Translation Editor.     

The dynamics of excitons and trions in resonant tunneling diodes

The aim of this work is to study the dynamic formation and dissociation of trions and excitons in double barrier resonant tunneling diodes. We propose a system of rate equations that takes into account the formation, dissociation and annihilation of these complexes inside the quantum well. From the solutions of the coupled equations, we are able to study the modulation of excitons and trions formation in the device as a function of the applied bias. The results of our model agree qualitatively with the experiments showing the viability of these rate equations system to study the dynamics of complex systems.     

Identification of excitons,trions and biexcitons in single‐layer WS2

Single‐layer WS₂ is a direct‐gap semiconductor showing strong excitonic photoluminescence features in the visible spectral range. Here, we present temperature‐dependent photoluminescence measurements on mechanically exfoliated single‐layer WS₂, revealing the existence of neutral and charged excitons at low temperatures as well as at room temperature. By applying a gate voltage, we can electrically control the ratio of excitons and trions and assert a residual n‐type doping of our samples. At high excitation densities and low temperatures, an additional peak at energies below the trion dominates the photoluminescence, which we identify as biexciton emission. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Trions,molecules and excitons above the Mott density in Ge

Measurements of the luminescence from intrinsic Ge, with a nearly uniform photoexcited carrier density, indicate the presence of trions, molecules and excitons at temperatures between 5.5 K and 15 K. We do not observe an ionization catastrophe at densities above the Mott criterion -- an observation which suggests large quantum corrections to the Debye-Huckel screening model.     

Polarization anisotropy of exciton in self-assembled elliptical InP/InGaP quantum dots

Optical anisotropy of self-assembled elliptical InP quantum dots has been investigated in terms of the polarization dependence of excitons. Although large size inhomogeneity is present, two kinds of characteristic quantum dots, which are classified into large and small quantum dots, were found in terms of the polarization anisotropy. We have confirmed that the large quantum dots are more pronounced in the polarization anisotropy, where the degree of linear polarization for the large quantum dots is significantly larger (∼60%) than that for the small ones (∼36%). The effective shape of quantum dots is also estimated by using the size dependence of oscillator strength, which is in agreement with the AFM image. We also suggest that the anisotropy of exciton oscillator strength can be modified via the dipole–dipole interaction between nearest exciton dipoles.     

Indirect excitons and double electron-hole layers in a wide single GaAs/AlGaAs quantum well in a strong electric field

The recombination spectra of indirect excitons and double electron-hole layers in a wide single quantum well in an electric field are studied. It is found that electrons and holes in the wide well become spatially separated in a sufficiently strong electric field. This leads to a substantial reorganization of the radiative recombination spectrum and to a significant increase in the carrier lifetime. It is shown that the total charge of the electron-hole system can be changed by varying the photoexcitation frequency and the applied electric field, thus passing from the neutral case of indirect excitons to the case of charged double electron-hole layers. The concentration of excess carriers in the well is measured as a function of the electric field strength. The behavior of the excited states of indirect heavy-hole and light-hole excitions is studied for a neutral excitonic system in a strong electric field. It is shown that the electric-field dependences allow the excited states of indirect excitons with a light hole to be distinguished from the excited states with a heavy hole.     

Spin-dependent coexistence of weakly coupled and strongly coupled modes in semiconductor microcavities

The dependence of the transition from the strong-coupling regime to the weak-coupling regime on the polariton spin orientation in a InGaAs semiconductor microcavity is experimental studied by means of time-resolved photoluminescence. Polaritons are created by non-resonant circularly-polarized optical excitation and the power intensity that breaks the strong coupling is found to be much lower for co-polarized polaritons than that for cross-polarized polaritons. Coulomb screening effects alone cannot explain the stronger loss of oscillator strength for majority excitons (co-polarized) and spin-dependent mechanisms are required to justify such behaviour.     

Charged and neutral excitonic complexes in GaAs/AlGaAs quantum wells

The temperature and magnetic-field dependences of the recombination line of multiparticle excitonic complexes in undoped and lightly doped GaAs/AlGaAs quantum wells are investigated. These dependences have previously been attributed to free charged excitons (trions). It is shown that this line corresponds to a bound state of a complex, specifically, to an exciton bound on a neutral donor in a barrier. It is found that as the temperature or pump power is raised, there appear in the recombination spectrum not only a cyclotron replica shifted downward in energy but also a replica which is symmetrically shifted upwards in energy by an amount equal to the cyclotron energy and which is due to emission from an excited state of an impurity complex. The behavior of the cyclotron replicas is studied as a function of the electron density and temperature. Pis’ma Zh. éksp. Teor. Fiz. 66, No. 11, 730–735 (10 December 1997)     

电子关联对聚乙炔中激子类型的影响

在SSH哈密顿基础上引进电子关联,对反式聚乙炔链中光致激子的产生和演化过程实施分子动力学模拟。弱关联强度U取值0～1.250 eV,V =U/2取值0～0.625 eV .计算结果表明,关联强度的大小影响链中元激发类型,U＜0.555eV时产生的元激发为孤子-反孤子对,U ＞0.555eV 时产生的元激发为正负荷电极化子对。为进一步讨论该类型一维系统中不同类型激子的产生、输运、衰减等动态过程,关联强度U的选择提供参考。     

电场对高分子中极化子激子的影响

介绍了近年来有关外电场对高分子中极化子激子影响的研究工作。它们包括 :研究方法 ,外电场注入的或光激发引起的电子和空穴会在高分子中形成极化子激子 ,弱或中等强度电场使极化子激子极化 ,强电场解离极化子激子 ,发现高分子中极化子双激子具有反向极化新性质 ,探讨反向极化这个新的物理现象的物理起因、意义及可能的应用。